Source : Webster's Revised Unabridged Dictionary (1913)

Alliterate \Al*lit"er*ate\, v. t.
   To employ or place so as to make alliteration. --Skeat.

Alliterate \Al*lit"er*ate\, v. i.
   To compose alliteratively; also, to constitute alliteration.

Source : WordNet®

alliterate
     v : use alliteration as a form of poetry